Hierarchical magnetic nanoparticle-enzyme mesoporous assemblies embedded in macroporous scaffolds

Abstract

A hierarchical catalyst composition comprising a continuous or particulate macroporous scaffold in which is incorporated mesoporous aggregates of magnetic nanoparticles, wherein an enzyme is embedded in mesopores of the mesoporous aggregates of magnetic nanoparticles. Methods for synthesizing the hierarchical catalyst composition are also described. Also described are processes that use the recoverable hierarchical catalyst composition for depolymerizing lignin, remediation of water contaminated with aromatic substances, polymerizing monomers by a free-radical mechanism, epoxidation of alkenes, halogenation of phenols, inhibiting growth and function of microorganisms in a solution, and carbon dioxide conversion to methanol. Further described are methods for increasing the space time yield and / or total turnover number of a liquid-phase chemical reaction that includes magnetic particles to facilitate the chemical reaction, the method comprising subjecting the chemical reaction to a plurality of magnetic fields of selected magnetic strength, relative position in the chemical reaction, and relative motion.

Description

CROSS-REFERENCE TO RELATED APPLICATIONS[0001]This application claims priority from U.S. Provisional Application No. 61 / 710,110, filed Oct. 5, 2012, and U.S. Provisional Application No. 61 / 767,477, filed Feb. 21, 2013, both of which are herein incorporated by reference in their entirety.STATEMENT REGARDING FEDERALLY SPONSORED RESEARCH[0002]This invention was made with government support under contract to the Northeast Sun Grant Initiative at Cornell University US Department of Transportation Assistance #DTOS59-07-G-00052. The government has certain rights in the invention.BACKGROUND OF THE DISCLOSURE[0003]Peroxidases (EC 1.11.1) are widely found in biological systems and form a subset of oxidoreductases that reduce hydrogen peroxide (H2O2) to water in order to oxidize a large variety of aromatic compounds ranging from phenol to aromatic amines. The reaction cycle of peroxidases is quite complex and begins with activation of heme by H2O2 to form the two-electron activated Compound I (...

AI Technical Summary

Benefits of technology

This patent describes a new way to make bionanocatalysts that combine an enzyme with magnetic nanoparticles to enhance their activity. These bionanocatalysts have faster turnover and lower inhibition compared to the free enzyme or magnetic nanoparticle clusters without enzyme. The size and magnetization of the MNPs affect the formation and structure of the bionanocatalysts. The patent also describes a method to increase the space time yield and total turnover number of a liquid-phase chemical reaction using the bionanocatalysts. The larger size and mass magnetization of the bionanocatalysts make them easier to capture, use, and remove from the reaction. This simplifies the re-use of the catalysts. Overall, this patent introduces a new and improved way to create highly efficient and easily removable enzymatic catalysts.

Problems solved by technology

Therefore, the complex kinetics associated with peroxidase enzymes can restrict their use in many processes and bioprocesses.

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